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Title: Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbB r 3 and CsPbC l 3

Abstract

The ternary compounds CsPbX3 (X = Br or Cl) have perovskite structures that are being considered for optical and electronic applications such as lasing and gamma-ray detection. An above-band-gap excitonic photoluminescence (PL) band is seen in both CsPbX3 compounds. An excitonic emission peak centered at 2.98 eV, ~0.1 eV above the room-temperature band gap, is observed for CsPbCl3. The thermal quenching of the excitonic luminescence is well described by a two-step quenching model, yielding activation energies of 0.057 and 0.0076 eV for high- and low-temperature regimes, respectively. CsPbBr3 exhibits bound excitonic luminescence peaks located at 2.29 and 2.33 eV that are attributed to recombination involving Br vacancy centers. Activation energies for thermal quenching of the excitonic luminescence of 0.017 and 0.0007 eV were calculated for CsPbBr3. Temperature-dependent PL experiments reveal unexpected blueshifts for all excitonic emission peaks in CsPbX3 compounds. A phonon-assisted step-up process leads to the blueshift in CsPbBr3 emission, while there is a contribution from band-gap widening in CsPbCl3. Finally, the absence of significant deep level defect luminescence in these compounds makes them attractive candidates for high-resolution, room-temperature radiation detection.

Authors:
 [1];  [1];  [2];  [3];  [1];  [1];  [2];  [3];  [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Material Science and Engineering
  2. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1494838
Alternate Identifier(s):
OSTI ID: 1234041
Grant/Contract Number:  
NA0002522; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 92; Journal Issue: 23; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; photoluminescence (PL); exciton emission; gamma-ray detection; perovskite halides; CsPbBr3; CsPbCl3

Citation Formats

Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., and Wessels, B. W. Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3. United States: N. p., 2015. Web. doi:10.1103/PhysRevB.92.235210.
Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., & Wessels, B. W. Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3. United States. doi:https://doi.org/10.1103/PhysRevB.92.235210
Sebastian, M., Peters, J. A., Stoumpos, C. C., Im, J., Kostina, S. S., Liu, Z., Kanatzidis, M. G., Freeman, A. J., and Wessels, B. W. Tue . "Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3". United States. doi:https://doi.org/10.1103/PhysRevB.92.235210. https://www.osti.gov/servlets/purl/1494838.
@article{osti_1494838,
title = {Excitonic emissions and above-band-gap luminescence in the single-crystal perovskite semiconductors CsPbBr3 and CsPbCl3},
author = {Sebastian, M. and Peters, J. A. and Stoumpos, C. C. and Im, J. and Kostina, S. S. and Liu, Z. and Kanatzidis, M. G. and Freeman, A. J. and Wessels, B. W.},
abstractNote = {The ternary compounds CsPbX3 (X = Br or Cl) have perovskite structures that are being considered for optical and electronic applications such as lasing and gamma-ray detection. An above-band-gap excitonic photoluminescence (PL) band is seen in both CsPbX3 compounds. An excitonic emission peak centered at 2.98 eV, ~0.1 eV above the room-temperature band gap, is observed for CsPbCl3. The thermal quenching of the excitonic luminescence is well described by a two-step quenching model, yielding activation energies of 0.057 and 0.0076 eV for high- and low-temperature regimes, respectively. CsPbBr3 exhibits bound excitonic luminescence peaks located at 2.29 and 2.33 eV that are attributed to recombination involving Br vacancy centers. Activation energies for thermal quenching of the excitonic luminescence of 0.017 and 0.0007 eV were calculated for CsPbBr3. Temperature-dependent PL experiments reveal unexpected blueshifts for all excitonic emission peaks in CsPbX3 compounds. A phonon-assisted step-up process leads to the blueshift in CsPbBr3 emission, while there is a contribution from band-gap widening in CsPbCl3. Finally, the absence of significant deep level defect luminescence in these compounds makes them attractive candidates for high-resolution, room-temperature radiation detection.},
doi = {10.1103/PhysRevB.92.235210},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 23,
volume = 92,
place = {United States},
year = {2015},
month = {12}
}

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Cited by: 33 works
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Figures / Tables:

Table 1 Table 1: Crystal data and structure refinement for CsPbCl3 at 293(2) K. 364

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